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Ethanol Dehydrogenation over Copper-Silica Catalysts: From Sub-Nanometer Clusters to 15 nm Large Particles
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SYSNO ASEP 0574069 Document Type J - Journal Article R&D Document Type Journal Article Subsidiary J Článek ve WOS Title Ethanol Dehydrogenation over Copper-Silica Catalysts: From Sub-Nanometer Clusters to 15 nm Large Particles Author(s) Pokorný, T. (CZ)
Vykoukal, V. (CZ)
Machač, P. (CZ)
Moravec, Z. (CZ)
Scotti, N. (IT)
Roupcová, Pavla (UFM-A) RID, ORCID
Karásková, K. (CZ)
Stýskalík, A. (CZ)Number of authors 8 Source Title ACS Sustainable Chemistry & Engineering. - : American Chemical Society - ISSN 2168-0485
Roč. 11, č. 30 (2023), s. 10980-10992Number of pages 13 s. Language eng - English Country US - United States Keywords ethanol dehydrogenation ; copper ; nanoparticles ; acetaldehyde ; sol-gel ; dry impregnation Subject RIV CF - Physical ; Theoretical Chemistry OECD category Particles and field physics Method of publishing Open access Institutional support UFM-A - RVO:68081723 UT WOS 001033052800001 EID SCOPUS 85166773876 DOI 10.1021/acssuschemeng.2c06777 Annotation Comparison of four preparation methodsshowed that the simpleand cost-effective dry impregnation provides Cu/SiO2 materialshowing the most stable catalytic behavior in potential renewableacetaldehyde production despite having a broad particle size distribution.
Non-oxidative ethanoldehydrogenation is a renewable source ofacetaldehyde and hydrogen. The reaction is often catalyzed by supportedcopper catalysts with high selectivity. The activity and long-termstability depend on many factors, including particle size, choiceof support, doping, etc. Herein, we present four different syntheticpathways to prepare Cu/SiO2 catalysts (& SIM,2.5 wt %Cu) with varying copper distribution: hydrolytic sol-gel (sub-nanometerclusters), dry impregnation (A ̅ = 3.4 nm, & sigma,= 0.9 nm and particles up to 32 nm), strong electrostatic adsorption(A ̅ = 3.1 nm, & sigma, = 0.6 nm), and solvothermalhot injection followed by Cu particle deposition (A ̅ = 4.0 nm, & sigma, = 0.8 nm). All materials were characterized byICP-OES, XPS, N-2 physisorption, STEM-EDS, XRD, RFC N2O, and H-2-TPR and tested in ethanol dehydrogenationfrom 185 to 325 & DEG,C. The sample prepared by hydrolytic sol-gelexhibited high Cu dispersion and, accordingly, the highest catalyticactivity. Its acetaldehyde productivity (2.79 g g(-1) h(-1) at 255 & DEG,C) outperforms most of the Cu-basedcatalysts reported in the literature, but it lacks stability and tendsto deactivate over time. On the other hand, the sample prepared bysimple and cost-effective dry impregnation, despite having Cu particlesof various sizes, was still highly active (2.42 g g(-1) h(-1) acetaldehyde at 255 & DEG,C). Importantly,it was the most stable sample out of the studied materials. The characterizationof the spent catalyst confirmed its exceptional properties: it showedthe lowest extent of both coking and particle sintering.Workplace Institute of Physics of Materials Contact Yvonna Šrámková, sramkova@ipm.cz, Tel.: 532 290 485 Year of Publishing 2024 Electronic address https://pubs.acs.org/doi/10.1021/acssuschemeng.2c06777
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